CN101899320A - Catalytic conversion method for producing high cetane number light diesel oil - Google Patents
Catalytic conversion method for producing high cetane number light diesel oil Download PDFInfo
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Abstract
The invention relates to a catalytic conversion method for producing high cetane number light diesel oil, which comprises the following steps: contacting raw oil with a catalyst containing macroporous zeolite in a reactor to react, wherein the reaction temperature, the oil gas residence time and the weight ratio of the catalyst to the raw oil are sufficient to obtain the reaction product in which catalytic wax oil accounts for 12-60 wt% of the raw oil, the oil gas residence time is 0.1-5 seconds, the reaction temperature is 420-550 DEG C, and the weight ratio of the catalyst to the raw oil is 1-10; maximally and selectively cracking alkanes, alkyl aromatic side chains and the like in the raw material to enter the light diesel oil fraction of the product, thereby ensuring that the main component in the light diesel oil fraction is the alkanes; and finally, the directly producing high cetane number light diesel oil through catalytic cracking.
Description
Technical field
The present invention relates to a kind of catalysis conversion method that improves catalytic cracking solar oil quality.More particularly, be the method that improves catalytic cracking solar oil cetane value by catalytic cracking substantially.
Background technology
Demand to high-quality diesel oil in worldwide increases day by day, to the then minimizing day by day of demand of oil fuel.Though vapour, diesel oil increase in demand are different and different with the area, generally worldwide will be above to the gasoline demand rate of growth to diesel oil growth of requirement speed.Therefore, more low-cetane catalysis solar oil just is being used to the blend component as diesel oil.And, need carry out upgrading to the catalysis solar oil in order to satisfy the demand of high-quality diesel oil, perhaps directly produce a large amount of high-quality catalysis solar oils by catalytic cracking (FCC).
In the prior art, the method for catalysis solar oil upgrading is mainly comprised hydrotreatment and alkylation, but these method costs are higher.
Another method is directly to improve the quality of catalysis solar oil in catalytic cracking process.CN101171063A has disclosed a kind of improvement and has been suitable as the FCC method of diesel oil fuel with the distillate quality of mixed oil.This method combines the inter-stage molecular separation of segmentation FCC conversion process and polycyclic aromatic hydrocarbons species.The low and higher reaction zone of harshness improves the output of diesel quality overhead product with the selectivity molecular separation in the lifter of FCC reactor.But this method Special attention will be given to obtains the diesel oil distillate of the high hexadecane value of enriched saturated hydrocarbon by membrane sepn.
Summary of the invention
The objective of the invention is to provide on the basis of existing technology a kind of catalysis conversion method of producing high cetane number light diesel oil.
The catalysis conversion method of production high cetane number light diesel oil provided by the invention comprises:
Stock oil contacts with the catalyzer that contains large pore zeolite in reactor and reacts, the weight ratio of temperature of reaction, the oil gas residence time, catalyzer and stock oil is enough to make reaction to obtain comprising the reaction product that accounts for stock oil 12～60 heavy % catalytic wax oil, the wherein said oil gas residence time is 0.1～5 second, described temperature of reaction is 420～550 ℃, and described catalyzer and stock oil weight ratio are 1～10.
Described stock oil is selected from or comprises petroleum hydrocarbon and/or other mineral oil, wherein petroleum hydrocarbon is selected from one or more the mixture in vacuum gas oil, atmospheric gas oil, coker gas oil, deasphalted oil, vacuum residuum, the long residuum, and other mineral oil is one or more the mixture in liquefied coal coil, tar sand oil, the shale oil.
Described catalyzer comprises zeolite, inorganic oxide, clay.In butt, each component accounts for total catalyst weight respectively: the heavy % in zeolite 5 heavy～40, the heavy % in preferred 10 heavy～30; The heavy % in inorganic oxide 0.5 heavy～50; The heavy % in clay 0 heavy～70.Its mesolite is lived as activity and is divided, and is selected from large pore zeolite.Described large pore zeolite is meant one or more the mixture in this group zeolite that the super steady Y that is obtained by Rare Earth Y, rare earth hydrogen Y, different methods, high silicon Y constitute.
Inorganic oxide is selected from silicon-dioxide (SiO as matrix
2) and/or aluminium sesquioxide (Al
2O
3).In butt, the heavy % in silica comprises 50 heavy～90 in the inorganic oxide, aluminium sesquioxide accounts for the heavy % in 10 heavy～50.
Clay is as caking agent, is selected from kaolin, halloysite, polynite, diatomite, halloysite, saponite, rectorite, sepiolite, attapulgite, hydrotalcite, the wilkinite one or more.
Preferred reaction conditions is as follows: 430～500 ℃ more preferably 430～480 ℃ of temperature of reaction; More preferably 0.8～3 second 0.5～4 second oil gas residence time; The weight ratio 1～8 of catalyzer and stock oil more preferably 1～6.
In a more preferred embodiment, reaction pressure is 0.10MPa～1.0MPa.
In a more preferred embodiment, described reactor be selected from riser tube, etc. one or more the combination in the fluidized-bed, isodiametric fluidized-bed, upstriker transfer limes, downstriker transfer limes of linear speed, or with the two or more combinations of a kind of reactor, described combination comprises series connection or/and in parallel, and wherein riser tube is the isodiametric riser tube of routine or the riser tube of various forms reducing.For riser tube, transfer limes reactor, described temperature of reaction is meant its temperature out; For fluidized-bed reactor, described temperature of reaction is meant its bed medial temperature.
In a more preferred embodiment, described stock oil is introduced in the reactor, or described stock oil is introduced in the reactor in the position of identical or different height more than a position.
In a more preferred embodiment, described method also comprises separates reaction product with catalyzer, and catalyzer is Returning reactor behind stripping, coke burning regeneration, and the product after the separation comprises high hexadecane value diesel oil and catalytic wax oil.
In a more preferred embodiment, described catalytic wax oil is that initial boiling point is not less than 350 ℃ cut.
In a more preferred embodiment, described catalytic wax oil hydrogen richness is not less than 11.0 heavy %, preferably is not less than 11.5 heavy %.
In a more preferred embodiment, separating of heavy aromatics in the described catalytic wax oil and non-aromatics can be adopted the catalytic wax oil extraction plant, perhaps catalytic wax oil is as the stock oil of conventional catalytic cracking unit, and perhaps catalytic wax oil adopts the hydrogenation mode to enter the catalytic wax oil hydrogenation unit.
The catalytic wax oil extraction solvent is selected from methyl-sulphoxide, furfural, dimethyl formamide, monoethanolamine, ethylene glycol, 1, the mixture of one or more in the materials such as 2-propylene glycol.The extractive process solvent recovery cycle is used.Extraction temperature is 40～120 ℃, and the volume ratio between solvent and the raw material is 0.5～5.0.Extractum is one of a purpose product heavy aromatics, and it is non-aromatics as one of raw material of catalytic cracking that catalytic wax oil is raffinated oil.
Conventional catalytic cracking unit adopts conventional catalytic cracking catalyst, and conditions such as temperature of reaction, agent-oil ratio and the oil gas residence time are all identical with conventional catalytic cracking unit operation, and the Hydrocarbon Content by Catalytic Cracking Operation method is identical with the method that those of ordinary skills know.
The catalytic wax oil hydrogenation is under there is situation in hydrogen, contacts with hydrotreating catalyst, at hydrogen dividing potential drop 3.0～20.0MPa, 300～450 ℃ of temperature of reaction, hydrogen to oil volume ratio 300～2000v/v, volume space velocity 0.1～3.0h
-1Reaction conditions under to carry out hydrotreatment resultant.The hydrogenation catalyst wax oil is as the stock oil of catalytic cracking unit.
Compared with prior art, beneficial effect of the present invention is mainly reflected in following aspect: by the optimal control of processing parameter and catalyst property, farthest with the alkane in the raw material, alkylaromatic hydrocarbon side chain etc. optionally cracking enter in the product solar oil cut, mainly being alkane in the composition of guaranteeing the solar oil cut, thereby finally can realize by catalytic cracking direct production high cetane number light diesel oil.
Description of drawings
Accompanying drawing is the basic procedure synoptic diagram of the catalysis conversion method of production high cetane number light diesel oil provided by the invention.
Embodiment
Further specify method provided by the present invention below in conjunction with accompanying drawing, but therefore the present invention is not subjected to any restriction.
Accompanying drawing is the basic procedure synoptic diagram of the catalysis conversion method of production high cetane number light diesel oil provided by the invention.
Embodiments of the present invention are to carry out in a kind of reducing riser reactor, about the more detailed description of this reactor referring to CN1237477A.
As shown in drawings, regenerated catalyst is through regenerator sloped tube 12, be subjected to guiding valve 11 controls to enter pre lift zone 2, the pre-medium that promotes also enters pre lift zone 2 through pipeline 1, under the effect of pre-lifting medium, regenerated catalyst enters the reaction zone I of riser reactor 4 bottoms through pre lift zone 2, fcc raw material also enters the reaction zone I of riser reactor bottom through pipeline 3, contact with catalyzer, reaction, and go upward to reaction zone II, reacted finish mixture enters cyclonic separator 7 from the riser tube outlet, carry out gas solid separation by cyclonic separator 7, the oil gas after the separation advances settling vessel collection chamber 6.Be advanced into stripping stage 5 under the band charcoal reclaimable catalyst after reaction oil gas separates, adopt superheated vapour to carry out stripping at stripping stage 5, band Pd/carbon catalyst behind the stripping through inclined tube 8 to be generated, be subjected to guiding valve 9 control to enter revivifier 10 regeneration, the catalyzer after the regeneration through regenerator sloped tube 12, be subjected to guiding valve 11 controls to return pre lift zone 2 to recycle.
Reaction product oil gas in the collection chamber 6 enters follow-up separation system 14 through main oil gas piping 13, separates the dry gas that obtains and draws through pipeline 15; Separating the liquefied gas that obtains draws through pipeline 16; Separating the gasoline that obtains draws through pipeline 17; Separating the diesel oil that obtains draws through pipeline 18; Separating the catalytic wax oil that obtains draws through pipeline 19.
The catalytic wax oil of drawing from pipeline 19 can enter conventional catalytic cracking unit 20; Perhaps enter aromatic extraction unit 21, isolated heavy aromatics is drawn through pipeline 24, and catalytic wax oil is raffinated oil and returned riser tube through pipeline 23; Perhaps enter catalytic wax oil hydrogenation unit 22, isolate light constituent and draw through pipeline 25, hydrogenation heavy oil is through pipeline 26 Returning catalyticing cracking devices.
The following examples will be further specified the present invention, but not thereby limiting the invention.Employed raw material oil properties is listed in table 1 respectively in embodiment and the Comparative Examples.Among the embodiment the catalyst A of using and catalyst B be respectively self-control and commercially available, wherein catalyst B is conventional catalytic cracking catalyst, by the Shandong catalyst plant production of catalyzer branch office of Sinopec Group, trade names are MLC-500.
Employed catalyst A preparation method is summarized as follows among the embodiment:
Water glass solution and 1 liter of free acid that to dispose 2 liters of silica concentrations be 155g/L are 148g/L, Al
2O
3Content is the acidified aluminum sulfate solution of 20g/L, and above-mentioned two kinds of solution enter the flash mixer reaction simultaneously, obtain silicon sol.
Add 465g kaolin (Suzhou kaolin company, solid content 80 weight %) in the silicon sol of above-mentioned preparation, pulling an oar obtained kaolin-silicon sol in 1 hour.
Contain Al
2O
3The pseudo-boehmite of 124g (Shandong Aluminum Plant, Al
2O
3Content is 33 weight %) and the 450g deionized water mix making beating 30 minutes, adding 25 ml concns then is hydrochloric acid (acid/Al of 31 weight %
2O
3Mol ratio is 0.2) peptization, continue making beating 2 hours, adding the 656g molecular sieve content then is that the ground DASY0.0 molecular sieve of 32 weight % (is a kind of overstable gamma zeolite, produce by the Shandong catalyst plant, lattice constant is 2.445nm) slurries, pulled an oar 30 minutes, and obtained the mixed serum of pseudo-boehmite and molecular sieve.
Kaolin-silicon sol the slurries of above-mentioned preparation are mixed making beating 10 minutes with the pseudo-boehmite of above-mentioned preparation and the mixed serum of molecular sieve, obtain catalyst slurry, it is that 20～120 microns, silica content are that 29.9 weight %, kaolin content are that 35.9 weight %, alumina content are that 13.9 weight %, molecular sieve content are the particle of 20.3 weight % that the slurries that obtain are spray dried to diameter, and drying temperature is 180 ℃.To not having sodium ion for detecting, 150 ℃ of oven dry obtain the used catalyst A of the present invention with deionized water wash.
Embodiment 1
The present embodiment explanation is adopted method provided by the invention to carry out the selective cracking reaction and is produced high-quality solar oil situation.
The kitty cracker schema as shown in drawings, stock oil A is through the reaction zone I of pipeline 3 injecting lift pipe reactors, contact, react in the bottom of riser reactor with the catalyst A that promotes by water vapor, weight ratio at riser reactor inner catalyst A and stock oil A is 3: 1, the residence time of stock oil A in riser reactor is 1.6 seconds, and temperature of reaction is 450 ℃.Collection chamber pressure is 0.2 MPa, and oil gas comes out after the fractionating system that cyclonic separator enters the rear portion after separating from riser tube.And the reclaimable catalyst of band charcoal enters stripping stage, and the reclaimable catalyst behind the stripping goes revivifier regeneration, and the catalyzer after the regeneration returns riser reactor and recycles.Test conditions, test-results are listed in table 2, and diesel oil character is listed in table 3.
Comparative Examples 1
Employing is tested with the identical riser reactor of above-mentioned embodiment, and raw materials used oily A and catalyst A are all same as the previously described embodiments, and difference can not be catalytic wax oil, only goes out a small amount of heavy oil.
The pre-medium that promotes is similarly water vapor in this Comparative Examples.Vacuum gas oil injects from the lower pipelines 3 of riser reactor, and the reaction times of vacuum gas oil in riser reactor is 3 seconds, and agent-oil ratio is 6: 1, and temperature of reaction is 500 ℃.The same embodiment of other condition.Test-results is listed in table 2, and diesel oil character is listed in table 3.
As can be seen from Table 2, the diesel yield of embodiment 1 is higher 11.18 percentage points than Comparative Examples 1; As can be seen from Table 3, the diesel oil alkane content of embodiment 1 is up to 55.2, and is higher 31.2 percentage points than Comparative Examples 1; The diesel cetane-number of embodiment 1 is up to 51, than Comparative Examples 1 high 24 units.
The present embodiment explanation is adopted method provided by the invention to carry out the selective cracking reaction and is produced high-quality solar oil situation.
The kitty cracker schema as shown in drawings, stock oil B is through pipeline 3 injecting lift pipe reactors, contact, react in the bottom of riser reactor with the catalyst B that promotes by water vapor, weight ratio at riser reactor inner catalyst A and stock oil A is 2: 1, the residence time of stock oil A in riser reactor is 2.6 seconds, and temperature of reaction is 480 ℃.Collection chamber pressure is 0.2 MPa, and oil gas comes out after the fractionating system that cyclonic separator enters the rear portion after separating from riser tube.And the reclaimable catalyst of band charcoal enters stripping stage, and the reclaimable catalyst behind the stripping goes revivifier regeneration, and the catalyzer after the regeneration returns riser reactor and recycles.Test conditions, test-results are listed in table 2, and diesel oil character is listed in table 3.
Comparative Examples 2
Employing is tested with the identical riser reactor of above-mentioned embodiment, and raw materials used oily A and catalyst B are all same as the previously described embodiments, and difference can not be catalytic wax oil, only goes out a small amount of heavy oil.
The pre-medium that promotes is similarly water vapor in this Comparative Examples.Vacuum gas oil injects from the lower pipelines 3 of riser reactor, and the reaction times of vacuum gas oil in riser reactor is 3 seconds, and agent-oil ratio is 6: 1, and temperature of reaction is 505 ℃.The same embodiment of other condition.Test-results is listed in table 2, and diesel oil character is listed in table 2.
As can be seen from Table 2, the diesel yield of embodiment 2 is higher 11.5 percentage points than Comparative Examples 2; As can be seen from Table 3, the diesel oil alkane content of embodiment 2 is up to 53.2, and is higher 32.2 percentage points than Comparative Examples 2; The diesel cetane-number of embodiment 2 is up to 48, than Comparative Examples 2 high 23 units.
Table 1
| Type of feed | A | B |
| Density (20 ℃), kilogram/rice 3 | 858.6 | 902.9 |
| Kinematic viscosity (100 ℃), millimeter 2/ second | 4.9 | 13.9 |
| Carbon residue, heavy % | 0.03 | 4.0 |
| Total nitrogen, heavy % | 0.05 | 0.26 |
| Sulphur, heavy % | 0.06 | 0.13 |
| Carbon, heavy % | 86.3 | 86.86 |
| Hydrogen, heavy % | 13.64 | 12.86 |
| Heavy metal content, ppm | ||
| Nickel | ＜0.1 | 5.3 |
| Vanadium | ＜0.1 | 1.1 |
| Boiling range, ℃ | ||
| Initial boiling point | 290 | 308 |
| 10％ | 372 | 395 |
| 30％ | 415 | 440 |
| 50％ | 440 | 479 |
| 70％ | 470 | 550 |
| 90％ | 502 | / |
| Final boiling point | / | / |
Table 2
Table 3
Claims (13)
1. catalysis conversion method of producing high cetane number light diesel oil, it is characterized in that stock oil contacts with the catalyzer that contains large pore zeolite in reactor reacts, the weight ratio of temperature of reaction, the oil gas residence time, catalyzer and stock oil is enough to make reaction to obtain comprising the reaction product that accounts for stock oil 12～60 heavy % catalytic wax oil, the wherein said oil gas residence time is 0.1～5 second, described temperature of reaction is 420～550 ℃, and described catalyzer and stock oil weight ratio are 1～10.
2. according to the method for claim 1, it is characterized in that described stock oil is selected from or comprises petroleum hydrocarbon and/or other mineral oil, wherein petroleum hydrocarbon is selected from one or more the mixture in vacuum gas oil, atmospheric gas oil, coker gas oil, deasphalted oil, vacuum residuum, the long residuum, and other mineral oil is one or more the mixture in liquefied coal coil, tar sand oil, the shale oil.
3. according to the method for claim 1, it is characterized in that described catalyzer comprises zeolite, inorganic oxide, clay, in butt, each component accounts for total catalyst weight respectively: the heavy % in zeolite 5 heavy～40, the heavy % in preferred 10 heavy～30; The heavy % in inorganic oxide 0.5 heavy～50; The heavy % in clay 0 heavy～70.
4. according to the method for claim 3, it is characterized in that described zeolite is selected from large pore zeolite, described large pore zeolite is meant one or more the mixture in this group zeolite that the super steady Y that is obtained by Rare Earth Y, rare earth hydrogen Y, different methods, high silicon Y constitute.
5. according to the method for claim 3, it is characterized in that described inorganic oxide is selected from silicon-dioxide and/or aluminium sesquioxide, in butt, the heavy % in silica comprises 50 heavy～90 in the inorganic oxide, aluminium sesquioxide accounts for the heavy % in 10 heavy～50.
6. according to the method for claim 3, it is characterized in that described clay is selected from one or more in kaolin, halloysite, polynite, diatomite, halloysite, saponite, rectorite, sepiolite, attapulgite, hydrotalcite, the wilkinite.
7. according to the method for claim 1, it is characterized in that reaction conditions is: 430～500 ℃ of temperature of reaction, 0.5～4 second oil gas residence time, the weight ratio 1～8 of catalyzer and stock oil.
8. according to the method for claim 7, it is characterized in that reaction conditions is: 430～480 ℃ of temperature of reaction, 0.8～3 second oil gas residence time, the weight ratio 1～6 of catalyzer and stock oil.
9. according to the method for claim 1, it is characterized in that described reactor be selected from riser tube, etc. one or more the combination in the fluidized-bed, isodiametric fluidized-bed, upstriker transfer limes, downstriker transfer limes of linear speed, or with the two or more combinations of a kind of reactor, described combination comprises series connection or/and in parallel, and wherein riser tube is the isodiametric riser tube of routine or the riser tube of various forms reducing.
10. according to the method for claim 1, it is characterized in that described method also comprises separates reaction product with catalyzer, and catalyzer is Returning reactor behind stripping, coke burning regeneration, and the product after the separation comprises high hexadecane value diesel oil and catalytic wax oil.
11., it is characterized in that described catalytic wax oil is that initial boiling point is not less than 350 ℃ cut according to the method for claim 1.
12., it is characterized in that described catalytic wax oil hydrogen richness is not less than 11.0 heavy % according to the method for claim 1 or 11.
13., it is characterized in that described catalytic wax oil hydrogen richness is not less than 11.5 heavy % according to the method for claim 12.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102079985A (en) * | 2009-11-26 | 2011-06-01 | 中国石油化工股份有限公司 | Catalytic conversion method for producing high-cetane number light diesel oil |
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|---|---|---|---|---|
| CN1340595A (en) * | 2000-08-30 | 2002-03-20 | 中国石油化工股份有限公司 | Feeding method for catalytic cracking of hydrocarbon oil |
| CN101171063A (en) * | 2005-03-28 | 2008-04-30 | 埃克森美孚研究工程公司 | FCC process combining molecular separation with staged conversion |
| CN101205475A (en) * | 2006-12-22 | 2008-06-25 | 中国石油化工股份有限公司 | Hydrocarbons catalytic conversion method for preparing low olefin-content gasoline |
| CN101724430A (en) * | 2008-10-31 | 2010-06-09 | 中国石油化工股份有限公司 | Method for preparing light-weight fuel oil and propylene from inferior raw oil |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1340595A (en) * | 2000-08-30 | 2002-03-20 | 中国石油化工股份有限公司 | Feeding method for catalytic cracking of hydrocarbon oil |
| CN101171063A (en) * | 2005-03-28 | 2008-04-30 | 埃克森美孚研究工程公司 | FCC process combining molecular separation with staged conversion |
| CN101205475A (en) * | 2006-12-22 | 2008-06-25 | 中国石油化工股份有限公司 | Hydrocarbons catalytic conversion method for preparing low olefin-content gasoline |
| CN101724430A (en) * | 2008-10-31 | 2010-06-09 | 中国石油化工股份有限公司 | Method for preparing light-weight fuel oil and propylene from inferior raw oil |
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| CN102079985A (en) * | 2009-11-26 | 2011-06-01 | 中国石油化工股份有限公司 | Catalytic conversion method for producing high-cetane number light diesel oil |
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